CN115038196A - Honeycomb structure, electrically heated carrier, and exhaust gas purifying apparatus - Google Patents
Honeycomb structure, electrically heated carrier, and exhaust gas purifying apparatus Download PDFInfo
- Publication number
- CN115038196A CN115038196A CN202111469148.6A CN202111469148A CN115038196A CN 115038196 A CN115038196 A CN 115038196A CN 202111469148 A CN202111469148 A CN 202111469148A CN 115038196 A CN115038196 A CN 115038196A
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- CN
- China
- Prior art keywords
- honeycomb structure
- electrode layer
- electrically heated
- structure portion
- peripheral wall
- Prior art date
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Images
Classifications
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B3/00—Ohmic-resistance heating
- H05B3/02—Details
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
- F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
- F01N3/022—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters characterised by specially adapted filtering structure, e.g. honeycomb, mesh or fibrous
- F01N3/0222—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters characterised by specially adapted filtering structure, e.g. honeycomb, mesh or fibrous the structure being monolithic, e.g. honeycombs
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
- F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
- F01N3/023—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
- F01N3/027—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles using electric or magnetic heating means
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
- F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion ; Methods of operation or control of catalytic converters
- F01N3/2006—Periodically heating or cooling catalytic reactors, e.g. at cold starting or overheating
- F01N3/2013—Periodically heating or cooling catalytic reactors, e.g. at cold starting or overheating using electric or magnetic heating means
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- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
- F01N3/28—Construction of catalytic reactors
- F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
- F01N3/2825—Ceramics
- F01N3/2828—Ceramic multi-channel monoliths, e.g. honeycombs
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B3/00—Ohmic-resistance heating
- H05B3/02—Details
- H05B3/03—Electrodes
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B3/00—Ohmic-resistance heating
- H05B3/02—Details
- H05B3/06—Heater elements structurally combined with coupling elements or holders
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B3/00—Ohmic-resistance heating
- H05B3/10—Heating elements characterised by the composition or nature of the materials or by the arrangement of the conductor
- H05B3/12—Heating elements characterised by the composition or nature of the materials or by the arrangement of the conductor characterised by the composition or nature of the conductive material
- H05B3/14—Heating elements characterised by the composition or nature of the materials or by the arrangement of the conductor characterised by the composition or nature of the conductive material the material being non-metallic
- H05B3/148—Silicon, e.g. silicon carbide, magnesium silicide, heating transistors or diodes
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B3/00—Ohmic-resistance heating
- H05B3/40—Heating elements having the shape of rods or tubes
- H05B3/42—Heating elements having the shape of rods or tubes non-flexible
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N2240/00—Combination or association of two or more different exhaust treating devices, or of at least one such device with an auxiliary device, not covered by indexing codes F01N2230/00 or F01N2250/00, one of the devices being
- F01N2240/16—Combination or association of two or more different exhaust treating devices, or of at least one such device with an auxiliary device, not covered by indexing codes F01N2230/00 or F01N2250/00, one of the devices being an electric heater, i.e. a resistance heater
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N2330/00—Structure of catalyst support or particle filter
- F01N2330/06—Ceramic, e.g. monoliths
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B2203/00—Aspects relating to Ohmic resistive heating covered by group H05B3/00
- H05B2203/019—Heaters using heating elements having a negative temperature coefficient
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- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B2203/00—Aspects relating to Ohmic resistive heating covered by group H05B3/00
- H05B2203/022—Heaters specially adapted for heating gaseous material
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B2203/00—Aspects relating to Ohmic resistive heating covered by group H05B3/00
- H05B2203/022—Heaters specially adapted for heating gaseous material
- H05B2203/024—Heaters using beehive flow through structures
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B2214/00—Aspects relating to resistive heating, induction heating and heating using microwaves, covered by groups H05B3/00, H05B6/00
- H05B2214/03—Heating of hydrocarbons
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Abstract
The invention provides a honeycomb structure, an electrically heated carrier, and an exhaust gas purifying apparatus, which can reduce the resistance reduction range when the temperature rises, easily apply electric power constantly with the passage of time, and can restrain the temperature from rising sharply. A honeycomb structure (20) of the present invention comprises: a honeycomb structure section (10) having an outer peripheral wall (12) and partition walls (13), the partition walls (13) being disposed inside the outer peripheral wall (12) and partitioning a plurality of cells (16), the plurality of cells (16) extending from one end surface to the other end surface to form flow paths; and a pair of electrode layers (14a, 14b) that are provided on the surface of the outer peripheral wall (12) of the honeycomb structure section (10) so as to face each other with the center axis of the honeycomb structure section (10) therebetween, wherein the honeycomb structure section (10) is made of a ceramic having NTC characteristics, and the electrode layers (14a, 14b) are made of a material having PTC characteristics.
Description
Technical Field
The invention relates to a honeycomb structure, an electrically heated carrier, and an exhaust gas purifying apparatus.
Background
Patent document 1 below proposes the use of a honeycomb structure as an electrically heated carrier. A honeycomb structure is provided with: a cylindrical honeycomb structure section having an outer peripheral wall and porous partition walls which partition and form a plurality of cells; and a pair of electrode portions disposed on side surfaces of the honeycomb structure portion, the honeycomb structure serving as a catalyst carrier and configured to function also as a heater by application of a voltage. The partition wall and the outer peripheral wall are mainly composed of a silicon-silicon carbide composite material or silicon carbide, and the electrode portion is mainly composed of silicon carbide particles and silicon.
For example, as shown in patent document 2 and the like described below, silicon carbide is known to have a characteristic (NTC characteristic) in which the resistance decreases with an increase in temperature. The honeycomb structure disclosed in patent document 1 has NTC characteristics because the honeycomb structure portion and the electrode portion contain silicon carbide.
Documents of the prior art
Patent literature
Patent document 1: international publication No. 2011/125815
Patent document 2: japanese laid-open patent publication No. 7-89764
Disclosure of Invention
In the electrically heated carrier that functions as a heater by applying a voltage, it is not preferable that the resistance varies due to a temperature change from the viewpoint of temperature control of the electrically heated carrier. On the other hand, if the resistance variation due to the temperature change is small, the voltage and current applied to control the temperature are easily controlled. In addition, when the resistance is decreased to a large extent when the temperature of the electrically heated carrier is increased, the current is likely to flow, and the temperature of the electrically heated carrier may be rapidly increased. In particular, if the honeycomb structure portion having the NTC characteristic is employed, when the temperature of the honeycomb structure increases, the resistance decreases, and therefore, there is a possibility that the current excessively flows, resulting in a sharp increase in temperature.
The present invention has been made in view of the above problems, and an object thereof is to provide a honeycomb structure, an electrically heated carrier, and an exhaust gas purifying apparatus, which can reduce the resistance drop width at the time of temperature rise, facilitate constant application of electric power with the passage of time, and suppress a rapid temperature rise.
The honeycomb structure according to the present invention includes: a honeycomb structure section having an outer peripheral wall and partition walls arranged inside the outer peripheral wall and partitioning a plurality of cells extending from one end surface to the other end surface to form flow paths; and a pair of electrode layers provided on the surface of the outer peripheral wall of the honeycomb structure portion so as to face each other with the center axis of the honeycomb structure portion interposed therebetween, wherein the honeycomb structure portion is made of a ceramic having NTC characteristics, and the electrode layers are made of a material having PTC characteristics.
The electrically heated carrier according to the present invention comprises: the above-described honeycomb structure; and an electrode terminal electrically connected to the electrode layer of the honeycomb structure.
The present invention relates to an exhaust gas purification device comprising: the above-mentioned electrically heated carrier; and a tank for holding the electrically heated carrier.
Effects of the invention
According to the honeycomb structure, the electrically heated carrier, and the exhaust gas purifying apparatus of the present invention, since the honeycomb structure portion is made of ceramic having NTC characteristics and the electrode layer is made of a material having PTC characteristics, the resistance drop width at the time of temperature rise can be reduced, electric power can be applied easily and constantly with the passage of time, and a rapid temperature rise can be suppressed.
Drawings
Fig. 1 is an external view of a honeycomb structure according to an embodiment of the present invention.
Fig. 2 is a schematic cross-sectional view of an electrode layer provided on a honeycomb structure portion of an electrically heated carrier and an electrode terminal provided on the electrode layer, the cross-sectional view being perpendicular to the direction in which cells extend.
Description of the reference numerals
10 … honeycomb structure part, 12 … peripheral wall, 13 … partition wall, 14a, 14b … electrode layer, 15a, 15b … electrode terminal, 16 … cell, 20 … honeycomb structure body, 30 … electrical heating carrier.
Detailed Description
Embodiments of the honeycomb structure, the electrically heated carrier, and the exhaust gas purifying apparatus according to the present invention will be described below with reference to the drawings, but the present invention is not limited to the embodiments, and various changes, modifications, and improvements can be made based on the knowledge of those skilled in the art without departing from the scope of the present invention.
< honeycomb structure and electrically heated carrier >
Fig. 1 is a schematic external view of a honeycomb structure 20 according to an embodiment of the present invention. Fig. 2 is a schematic cross-sectional view of the electrode layers 14a and 14b provided on the honeycomb structure portion 10 of the electrically heated carrier 30 and the electrode terminals 15a and 15b provided on the electrode layers 14a and 14b, respectively, perpendicular to the extending direction of the cells 16 according to the embodiment of the present invention.
(1. Honeycomb structure)
The honeycomb structure 20 includes a honeycomb structure portion 10 and a pair of electrode layers 14a and 14 b. The honeycomb structure portion 10 is a ceramic columnar member having an outer peripheral wall 12 and partition walls 13, the partition walls 13 being disposed inside the outer peripheral wall 12 and partitioning a plurality of cells 16, the cells 16 extending from one end face to the other end face to form flow paths. The columnar shape can be understood as: has a three-dimensional shape with a thickness in the extending direction of the cells 16 (the axial direction of the honeycomb structural portion 10). The ratio (aspect ratio) of the axial length of the honeycomb structure portion 10 to the diameter or width of the end face of the honeycomb structure portion 10 is arbitrary. The columnar shape may include a shape (flat shape) in which the axial length of the honeycomb structure portion 10 is smaller than the diameter or width of the end face.
The outer shape of the honeycomb structural portion 10 is not particularly limited as long as it is columnar, and for example, it may be columnar (columnar shape) with a circular end face, columnar with an elliptical end face, or polygonal (quadrangular, pentagonal) end facePolygonal, hexagonal, heptagonal, octagonal, etc.) columnar, etc. In addition, the size of the honeycomb structure portion 10 is preferably 2000 to 20000mm in the area of the end face for the reason of improving heat resistance (suppressing occurrence of cracks in the outer peripheral wall in the circumferential direction) 2 More preferably 5000 to 15000mm 2 。
The shape of the cells in a cross section perpendicular to the direction of extension of the cells 16 is not limited, and is preferably a quadrangle, a hexagon, an octagon, or a combination of these shapes. Among them, when the honeycomb structure portion 10 is used as a catalyst carrier and carries a catalyst, it is more preferable that the catalyst has a rectangular shape and a hexagonal shape which can reduce the pressure loss during the exhaust gas flow and can improve the purification performance of the catalyst. From the viewpoint of making the purification performance of the catalyst more excellent, a hexagonal shape is more preferable.
The thickness of the partition wall 13 defining the compartment 16 is preferably 0.1 to 0.3mm, and more preferably 0.1 to 0.2 mm. The thickness of the partition walls 13 is 0.1mm or more, and the strength of the honeycomb structure portion 10 can be suppressed from being lowered. The thickness of the partition walls 13 is 0.3mm or less, and it is possible to suppress an increase in pressure loss when exhaust gas flows when the honeycomb structure portion 10 is used as a catalyst carrier and a catalyst is carried. In the present invention, the thickness of the partition wall 13 is defined as: a length of a portion passing through the partition wall 13 in a line segment connecting the centers of gravity of the adjacent compartments 16 to each other in a cross section perpendicular to the extending direction of the compartments 16.
In the honeycomb structure portion 10, the cell density is preferably 40 to 150 cells/cm in a cross section perpendicular to the extending direction of the cells 16 2 More preferably 70 to 100 compartments/cm 2 . By setting the cell density in such a range, the purification performance of the catalyst can be improved while reducing the pressure loss during the exhaust gas flow. If the cell density is 40 cells/cm 2 As described above, the catalyst supporting area can be sufficiently ensured. If the cell density is 150 cells/cm 2 Hereinafter, when the honeycomb structure portion 10 is used as a catalyst carrier and a catalyst is carried thereon, an increase in pressure loss during exhaust gas flow can be suppressed. The cell density is: one of the honeycomb-structure portions 10 except for the outer peripheral wall 12 portionThe area of each end face portion divided by the number of compartments.
It is useful to provide the outer peripheral wall 12 in the honeycomb structure portion 10 from the viewpoint of ensuring the structural strength of the honeycomb structure portion 10 and suppressing the leakage of the fluid flowing through the cells 16 from the outer peripheral wall 12. Specifically, the thickness of the outer peripheral wall 12 is preferably 0.05mm or more, more preferably 0.10mm or more, and still more preferably 0.15mm or more. However, if the outer peripheral wall 12 is too thick, the strength becomes too high, the strength becomes unbalanced with the partition wall 13, and the thermal shock resistance is lowered, so the thickness of the outer peripheral wall 12 is preferably 1.0mm or less, more preferably 0.7mm or less, and still more preferably 0.5mm or less. Here, the thickness of the outer peripheral wall 12 is defined as: the thickness in the normal direction of the tangent to the outer peripheral wall 12 at the measurement site when the site of the outer peripheral wall 12 whose thickness is to be measured is observed in a cross section perpendicular to the extending direction of the compartment.
The honeycomb structure portion 10 has electrical conductivity. The volume resistivity of the honeycomb structure 10 is not particularly limited as long as it can be electrically conducted and generates heat by joule heat, and is preferably 0.1 to 200 Ω · cm, and more preferably 1 to 200 Ω · cm. In the present invention, the volume resistivity of the honeycomb structure portion 10 is a value measured at a temperature of 25 ℃ by a four-terminal method.
The honeycomb structure portion 10 is made of a ceramic having NTC characteristics (characteristics in which resistance decreases with an increase in temperature). The NTC property includes, for example: the increase rate of the electrical resistance of the honeycomb structure portion described later exhibits a negative value or the like. The material of the honeycomb structure portion 10 is not limited, and may be selected from non-oxide ceramics such as silicon carbide, silicon nitride, and aluminum nitride. In addition, a silicon carbide-metal silicon composite material, a silicon carbide/graphite composite material, or the like can also be used. Among them, from the viewpoint of achieving both heat resistance and electrical conductivity, the material of the honeycomb structure portion 10 preferably contains a silicon-silicon carbide composite material or a ceramic containing silicon carbide as a main component. When the material of the honeycomb structure portion 10 is a silicon-silicon carbide composite material as a main component, it means that the honeycomb structure portion 10 contains 90 mass% or more of the silicon-silicon carbide composite material (total mass) of the entire structure. Here, the silicon-silicon carbide composite material contains silicon carbide particles as an aggregate and silicon as a bonding material for bonding the silicon carbide particles, and it is preferable that a plurality of the silicon carbide particles are bonded to each other through silicon so as to form pores between the silicon carbide particles. When the material of the honeycomb structure portion 10 contains silicon carbide as a main component, it means that the honeycomb structure portion 10 contains 90 mass% or more of silicon carbide (total mass) of the whole.
The rate of increase in the electrical resistance of the honeycomb structure 10 is preferably-80 to-10%. The rate of increase in the resistance of the honeycomb structure 10 can be determined by measuring the volume resistivity (Ω · cm) at 2 points at 50 ℃ and 500 ℃ by the four-terminal method, and dividing the value obtained by subtracting the volume resistivity at 50 ℃ from the volume resistivity at 500 ℃ by the volume resistivity at 50 ℃ and multiplying the result by 100. If the resistance increase rate is-80% or more, the resistance change during the energization heating can be reduced, and the electric power can be easily applied constantly with the passage of time during the energization. If the rate of increase in electrical resistance of the honeycomb structure portion 10 is-10% or less, the honeycomb structure portion 10 exhibits NTC characteristics, and a ceramic containing a silicon-silicon carbide composite material or silicon carbide as a main component may be used for the honeycomb structure portion 10. The rate of increase in the electrical resistance of the honeycomb structure 10 is more preferably from-70 to-20%, still more preferably from-70 to-30%.
The porosity of the honeycomb structure portion 10 is preferably higher than the porosity of the electrode layers 14a and 14 b. If the porosity satisfies this relationship, when the honeycomb structure 20 is used as a catalyst carrier and a catalyst is supported, the catalyst is easily supported by the honeycomb structure portion 10 having a high porosity, and it is difficult to support the catalyst on the electrode layers 14a and 14b having a low porosity. As a result, the catalyst can be effectively supported by the honeycomb structure portion 10 through which the exhaust gas passes, and the catalyst can be easily formed into a structure having excellent purification performance. The porosity of the honeycomb structure 10 is preferably 35 to 60%, more preferably 35 to 45%. The porosity is a value measured by a mercury porosimeter.
The thermal expansion coefficient of the honeycomb structure 10 is preferably 4.0 to 4.75ppm/K, and more preferably 4.0 to 4.6 ppm/K. The thermal expansion coefficient is: by the method according to JIS R1618: coefficient of linear thermal expansion of 40 to 800 ℃ measured by the method of 2002. As the thermal expansion meter, "TD 5000S (trade name)" manufactured by BrukerAXS may be used.
(2. electrode layer)
In the honeycomb structure 20, a pair of electrode layers 14a and 14b are provided on the surface of the outer peripheral wall 12 so as to face each other with the center axis of the honeycomb structure portion 10 interposed therebetween. The electrode layers 14a and 14b are made of a material having PTC characteristics (characteristics in which resistance increases with an increase in temperature). Examples of the PTC property include: the resistance increase rate of the electrode layer described later shows a positive value or the like.
In the honeycomb structure 20 and the electrically heated carrier 30 according to the embodiment of the present invention, since the honeycomb structure portion 10 is made of ceramic having NTC characteristics and the electrode layers 14a and 14b are made of material having PTC characteristics, the resistance balance of the entire electrically heated carrier can be controlled by controlling the resistances of the honeycomb structure portion 10 and the electrode layers 14a and 14b, and thus the honeycomb structure 20 and the electrically heated carrier 30 which can easily apply constant electric power to the electrically heated carrier with the passage of time can be obtained.
The thermal expansion coefficient of the electrode layers 14a and 14b is preferably larger than that of the honeycomb structure portion 10. If the thermal expansion coefficients satisfy the relationship, when the electrode layers 14a and 14b are provided with the electrode terminals 15a and 15b to form the electrically heated carrier 30, the difference in thermal expansion coefficients between the electrode layers 14a and 14b and the electrode terminals 15a and 15b is small, and the electrically heated carrier 30 having excellent thermal shock resistance is formed. The thermal expansion coefficient of the electrode layers 14a, 14b is preferably 4.5 to 10ppm/K, more preferably 4.5 to 7 ppm/K. The thermal expansion coefficients of the electrode layers 14a and 14b can be measured by the same method as the method for measuring the thermal expansion coefficient of the honeycomb structure portion 10 described above.
The electrode layers 14a and 14b preferably have a resistance increase rate of 2 to 40%. Similarly to the above-described increase rate of the resistance of the honeycomb structure portion 10, the increase rate of the resistance of the electrode layers 14a and 14b can be obtained by measuring the volume resistivity (Ω · cm) at 2 points at the temperatures of 50 ℃ and 500 ℃ by a four-terminal method, dividing the value obtained by subtracting the volume resistivity at 50 ℃ from the volume resistivity at 500 ℃ by the volume resistivity at 50 ℃ and multiplying the value by 100. If the resistance increase rate is 2% or more, the resistance of the electrode layers 14a and 14b increases due to the PTC characteristic when heated by energization, and the amount of resistance decrease of the honeycomb structure portion 10 which decreases due to the NTC characteristic when heated by energization is compensated, so that power can be easily applied constantly over time. If the rate of increase in the resistance of the electrode layers 14a and 14b is 40% or less, the amount of joule heat generated by the increase in the resistance of the electrode layers 14a and 14b during energization heating can be reduced. The resistance increase rate of the electrode layers 14a and 14b is more preferably 5 to 35%, and still more preferably 10 to 30%.
The electrode layers 14a and 14b may be made of a mixture of a metal and an oxide ceramic, or a mixture of a metal compound and an oxide ceramic. The metal may be a simple metal or an alloy, and examples thereof include: silicon, aluminum, iron, stainless steel, titanium, tungsten, Ni-Cr alloy, and the like. The metal compound is a metal oxide other than oxide ceramics, and examples thereof include: metal oxides, metal nitrides, metal carbides, metal silicides, metal borides, composite oxides, and the like. The metal or metal compound may be used alone or in combination of two or more. Examples of the oxide ceramic include: glass, cordierite, mullite, and the like. The oxide ceramics may be used alone or in combination of two or more. Among them, a mixture containing at least stainless steel and glass is more preferable in terms of easy adjustment of electric resistance and further excellent durability.
The material of the electrode layers 14a and 14b may be a mixture of carbon and ceramic. Examples of the ceramics include: glass, cordierite, mullite, silicon carbide, silicon nitride, zirconia, and the like. The ceramics may be used alone or in combination of two or more.
The formation regions of the electrode layers 14a and 14b are not particularly limited, and from the viewpoint of improving the uniform heat generation property of the honeycomb structure portion 10, it is preferable that the electrode layers 14a and 14b extend in a band shape on the outer surface of the outer peripheral wall 12 along the circumferential direction of the outer peripheral wall 12 and the extending direction of the cells. Specifically, from the viewpoint of facilitating the current to flow in the axial direction of the electrode layers 14a and 14b, the respective electrode layers 14a and 14b extend over 80% or more, preferably 90% or more, and more preferably the entire length between both end surfaces of the honeycomb structural portion 10. By forming the pair of electrode layers 14a and 14b in a band shape in this manner, a rapid temperature rise can be further easily suppressed. The reason for this is presumed to be: in a part of the honeycomb structure portion 10 having the NTC characteristic, the resistance is lowered, and if the temperature of the part is raised, the temperature of a part of the electrode layers 14a, 14b of the region close to the part of the honeycomb structure portion 10 is raised and the resistance is raised. Accordingly, it is considered that the temperature of the entire honeycomb structure portion 10 is uniformed because the current flows through the electrode layers 14a and 14b other than the electrode layers 14a and 14b, which are a part of the resistance increase, and then the current flows into the honeycomb structure portion 10.
The thickness of each electrode layer 14a, 14b is preferably 0.01 to 5mm, more preferably 0.01 to 3 mm. By setting the range as described above, the uniform heat generation property can be improved. If the thickness of each of the electrode layers 14a and 14b is 0.01mm or more, the resistance is appropriately controlled, and heat can be generated more uniformly. If the thickness of each of the electrode layers 14a and 14b is 5mm or less, the possibility of breakage at the time of can filling is reduced. The thickness of each electrode layer 14a, 14b is defined as: the thickness in the normal direction with respect to the tangent line at the measurement site of the outer surface of each electrode layer 14a, 14b when the site of the electrode layer 14a, 14b whose thickness is to be measured is observed in a cross section perpendicular to the extension direction of the cell.
(3. electrode terminal)
The electrode terminals 15a and 15b may be formed in a columnar shape, or may be formed in a plurality of branches in a comb-tooth shape, and have contact points connected to the electrode layers 14a and 14b at the respective branched portions. The electrode terminals 15a and 15b are disposed on the electrode layers 14a and 14b and electrically joined. Accordingly, if a voltage is applied to the electrode terminals 15a and 15b, the honeycomb structure portion 10 can be heated by joule heat by energization. Therefore, the honeycomb-structure portion 10 can also preferably function as a heater. The voltage to be applied is preferably 12 to 900V, more preferably 48 to 600V, and the voltage to be applied can be changed as appropriate.
The electrode terminals 15a and 15b may be made of metal. The metal may be a simple metal, an alloy, or the like, and is preferably an alloy containing at least one selected from the group consisting of Cr, Fe, Co, Ni, and Ti, and more preferably stainless steel and an Fe — Ni alloy, from the viewpoint of corrosion resistance, volume resistivity, and linear expansion coefficient. The shape and size of the electrode terminals 15a and 15b are not particularly limited, and may be appropriately designed according to the size of the electrically heated carrier, the energization performance, and the like.
The electrode terminals 15a, 15b may be made of ceramic. The ceramics include, but are not limited to: silicon carbide (SiC); tantalum silicide (TaSi) 2 ) And chromium silicide (CrSi) 2 ) Metal compounds such as metal silicides; and composite materials (cermets) containing one or more metals. Specific examples of the cermet include: a composite material of silicon and silicon carbide, a composite material of a metal silicide such as tantalum silicide and chromium silicide, and a metal silicon and silicon carbide, and further, from the viewpoint of reducing thermal expansion, a composite material obtained by adding one or more of alumina, mullite, zirconia, cordierite, silicon nitride, and an insulating ceramic such as aluminum nitride to one or more of the above-mentioned metals can be mentioned. The electrode terminals 15a and 15b may be made of the same material as the electrode layer.
When the electrode terminals 15a and 15b are ceramic terminals, the respective metal terminals may be joined to the tips thereof. The ceramic terminal and the metal terminal can be joined by caulking, welding, or using a conductive adhesive. As a material of the metal terminal, a conductive metal such as an iron alloy or a nickel alloy can be used.
The electrically heated carrier 30 can be used as a catalyst by supporting a catalyst on the electrically heated carrier 30. For example, a fluid such as automobile exhaust gas may be circulated through the flow paths of the plurality of compartments 16. Examples of the catalyst include: a noble metal-based catalyst or a catalyst other than a noble metal-based catalyst. Examples of the noble metal-based catalyst include: a three-way catalyst in which a noble metal such as platinum (Pt), palladium (Pd), or rhodium (Rh) is supported on the surface of pores of alumina and a co-catalyst such as cerium oxide or zirconium oxide is contained, an oxidation catalyst, or a NOx storage reduction catalyst (LNT catalyst) in which an alkaline earth metal and platinum are contained as storage components of nitrogen oxides (NOx). As the catalyst not using a noble metal, there can be exemplified: NOx selective reduction catalysts (SCR catalysts) containing copper-substituted zeolite or iron-substituted zeolite, and the like. In addition, two or more catalysts selected from the group consisting of these catalysts may be used. The method for supporting the catalyst is not particularly limited, and the catalyst may be supported by a conventional method for supporting the catalyst on the honeycomb structure.
< method for producing electrically heated Carrier
Next, a method for manufacturing the electrically heated carrier according to the present invention will be described by way of example. In one embodiment of the method for manufacturing an electrically heated carrier according to the present invention, the method includes: a step a1 of obtaining an unfired honeycomb structure with an electrode terminal forming paste; and a step A2 of firing the unbaked honeycomb structure with the electrode terminal forming paste to obtain a honeycomb structure with an electrode terminal. In another embodiment, the electrode layer forming paste and the electrode terminal forming paste may be baked and then attached to the honeycomb structure. In addition, in an embodiment in which the electrode terminal is made of metal, there are included: a step of obtaining a honeycomb structure by firing the unfired honeycomb structure with the electrode layer forming paste after obtaining the unfired honeycomb structure with the electrode layer forming paste; and a step of fixing the metal electrode terminal to the electrode layer of the honeycomb structure.
Step a1 is a step of preparing a columnar honeycomb formed body which is a precursor of the honeycomb structure, applying an electrode layer forming paste to the side surface of the columnar honeycomb formed body to obtain an unfired honeycomb structure with the electrode layer forming paste, and then providing an electrode terminal forming paste on the electrode layer forming paste to obtain the unfired honeycomb structure with the electrode terminal forming paste.
To produce the columnar honeycomb formed body, first, a metal silicon powder (metal silicon), a binder, a surfactant, a pore-forming material, water, and the like are added to a silicon carbide powder (silicon carbide) to produce a forming raw material. The mass of the metal silicon powder is preferably 10 to 40% by mass based on the total mass of the silicon carbide powder and the mass of the metal silicon powder. The average particle diameter of the silicon carbide particles in the silicon carbide powder (silicon carbide) is preferably 3 to 50 μm, and more preferably 3 to 40 μm. The average particle diameter of the metal silicon particles in the metal silicon powder (metal silicon) is preferably 2 to 35 μm. The average particle diameter of the silicon carbide particles and the metal silicon particles is: the arithmetic mean particle diameter on a volume basis in the frequency distribution of particle sizes was measured by a laser diffraction method.
Examples of the binder include: methylcellulose, hydroxypropyl methylcellulose, hydroxypropoxy cellulose, hydroxyethyl cellulose, carboxymethyl cellulose, polyvinyl alcohol, and the like. Among them, it is preferable to use both methylcellulose and hydroxypropyloxycellulose. The content of the binder is preferably 2.0 to 10.0 parts by mass, based on 100 parts by mass of the total mass of the silicon carbide powder and the metal silicon powder.
The water content is preferably 20 to 60 parts by mass, based on 100 parts by mass of the total of the silicon carbide powder and the metal silicon powder.
As the surfactant, ethylene glycol, dextrin, fatty acid soap, polyhydric alcohol, and the like can be used. These surfactants may be used alone or in combination of two or more. The content of the surfactant is preferably 0.1 to 2.0 parts by mass, based on 100 parts by mass of the total mass of the silicon carbide powder and the metal silicon powder.
The pore-forming material is not particularly limited as long as it forms pores after firing, and examples thereof include: graphite, starch, a foaming resin, a water-absorbent resin, silica gel, and the like. The content of the pore-forming material is preferably 0.5 to 10.0 parts by mass, based on 100 parts by mass of the total of the silicon carbide powder and the metal silicon powder. The average particle diameter of the pore-forming material is preferably 10 to 30 μm. The average particle size of the pore-forming material means: the arithmetic mean particle diameter on a volume basis in the frequency distribution of the particle size was measured by a laser diffraction method. When the pore-forming material is a water-absorbent resin, the average particle diameter of the pore-forming material is the average particle diameter after water absorption.
Next, the obtained molding raw material was kneaded to form a billet, and the billet was extrusion-molded to produce a columnar honeycomb molded body. In the extrusion molding, a die having a desired overall shape, cell shape, thickness of a partition wall, cell density, or the like may be used. Next, the obtained columnar honeycomb formed body is preferably dried. When the central axial direction length of the columnar honeycomb formed body is not a desired length, both bottom portions of the columnar honeycomb formed body may be cut to be a desired length. The dried columnar honeycomb formed body is referred to as a columnar honeycomb dried body.
Next, an electrode layer forming paste for forming an electrode layer was prepared. Various additives may be appropriately added to raw material powders (metal powders, glass powders, and the like) blended in accordance with the required characteristics of the electrode layer, and the mixture may be kneaded to form an electrode layer-forming paste. As the metal powder, metal powder such as stainless steel can be used.
Next, the obtained electrode layer forming paste was applied to the side surface of a columnar honeycomb formed body (typically, a columnar honeycomb dried body), thereby obtaining an unfired honeycomb structure with the electrode layer forming paste. The method of applying the electrode layer forming paste to the columnar honeycomb formed body can be performed based on a known method of manufacturing a honeycomb structure.
As a modification of the method for producing a honeycomb structure, in step a1, the columnar honeycomb formed body may be temporarily fired before the electrode layer forming paste is applied. That is, in this modification, a columnar honeycomb formed body is fired to produce a columnar honeycomb fired body, and an electrode layer is applied to the columnar honeycomb fired body to form a paste.
Next, in the case where the electrode terminal is composed of ceramic, an electrode terminal-forming paste for forming the electrode terminal is prepared. Various additives may be appropriately added to ceramic powder blended in accordance with the required characteristics of the electrode terminal and kneaded to form an electrode terminal-forming paste. Next, the prepared electrode terminal-forming paste was disposed in a columnar shape on the surface of the electrode layer on the honeycomb structure.
In step a2, the unbaked honeycomb structure with the electrode terminal forming paste is fired to obtain a honeycomb structure with an electrode terminal. The firing conditions can beThe sintering temperature is set to be below the atmospheric pressure under the inert gas atmosphere or the atmospheric atmosphere, the sintering temperature is 1150-1350 ℃, and the sintering time is 0.1-50 hours. For example, the firing atmosphere may be an inert gas atmosphere, and the pressure during firing may be normal pressure. In order to reduce the electrical resistance of the honeycomb structure portion 10, it is preferable to reduce the residual oxygen from the viewpoint of preventing oxidation, and it is preferable to set the atmosphere at the time of firing to 1.0 × 10 -4 After a high vacuum of Pa or more, the inert gas is purged and fired. Examples of the inert gas atmosphere include: n is a radical of 2 A gas atmosphere, a helium atmosphere, an argon atmosphere, and the like. The unfired honeycomb structure with the electrode terminal forming paste may be dried before firing. Before firing, degreasing may be performed to remove a binder and the like. Thus, an electrically heated carrier in which the electrode terminal and the electrode layer are electrically connected can be obtained.
When a metal terminal is used as the electrode terminal, the metal terminal is fixed to the electrode layer of the honeycomb structure 20. Examples of the fixing method include: laser welding, thermal spraying, ultrasonic welding, and the like.
< exhaust gas purifying apparatus >
The electrically heated carriers according to the embodiments of the present invention described above can be used in exhaust gas purification devices, respectively. The exhaust gas purifying apparatus includes an electrically heated carrier and a tank for holding the electrically heated carrier. In the exhaust gas purification device, an electrically heated carrier is provided in the middle of an exhaust gas flow path through which exhaust gas from an engine flows. As the tank body, a metal cylindrical member or the like that houses the electrically heated carrier can be used.
Claims (10)
1. A honeycomb structure, wherein,
the honeycomb structure is provided with:
a honeycomb structure portion having an outer peripheral wall and partition walls arranged inside the outer peripheral wall and partitioning a plurality of cells extending from one end surface to the other end surface to form flow paths; and
a pair of electrode layers provided on a surface of an outer peripheral wall of the honeycomb structure portion so as to face each other with a central axis of the honeycomb structure portion interposed therebetween,
the honeycomb structure portion is made of ceramic having NTC characteristics, and the electrode layer is made of a material having PTC characteristics.
2. The honeycomb structure body according to claim 1,
the porosity of the honeycomb structure portion is higher than the porosity of the electrode layer.
3. The honeycomb structure body according to claim 1 or 2,
the pair of electrode layers are respectively provided to extend along the extending direction of the compartment on the outer surface of the outer peripheral wall.
4. The honeycomb structure body according to any one of claims 1 to 3,
the rate of increase in resistance of the honeycomb structure portion is-80 to-10%.
5. The honeycomb structure body according to any one of claims 1 to 4,
the electrode layer has a thermal expansion coefficient larger than that of the honeycomb structure portion.
6. The honeycomb structure body according to any one of claims 1 to 5,
the resistance rise rate of the electrode layer is 2-40%.
7. The honeycomb structure body according to any one of claims 1 to 6,
the material of the electrode layer is a mixture of metal and oxide ceramic or a mixture of metal compound and oxide ceramic.
8. The honeycomb structure body according to any one of claims 1 to 6,
the electrode layer is made of a mixture of carbon and ceramic.
9. An electrically heated carrier, wherein,
the electrically heated carrier has:
the honeycomb structure body of any one of claims 1 to 8; and
an electrode terminal electrically connected to the electrode layer of the honeycomb structure.
10. An exhaust gas purifying device, wherein,
the exhaust gas purification device is provided with:
the electrically heated carrier of claim 9; and
a tank for holding the electrically heated carrier.
Applications Claiming Priority (4)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2021-033851 | 2021-03-03 | ||
| JP2021033851 | 2021-03-03 | ||
| JP2021-150525 | 2021-09-15 | ||
| JP2021150525A JP2022135885A (en) | 2021-03-03 | 2021-09-15 | Honeycomb structure, electrically heated carrier, and exhaust gas purification device |
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| CN115038196A true CN115038196A (en) | 2022-09-09 |
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| CN202111469148.6A Pending CN115038196A (en) | 2021-03-03 | 2021-12-03 | Honeycomb structure, electrically heated carrier, and exhaust gas purifying apparatus |
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| Country | Link |
|---|---|
| US (1) | US20220287154A1 (en) |
| CN (1) | CN115038196A (en) |
| DE (1) | DE102021213628A1 (en) |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| WO2020036067A1 (en) * | 2018-08-13 | 2020-02-20 | 日本碍子株式会社 | Heating element for heating passenger compartment, method of use thereof, and heater for heating passenger compartment |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH0789764A (en) | 1993-09-21 | 1995-04-04 | Tokai Konetsu Kogyo Co Ltd | Silicon carbide heating element |
| JP5663003B2 (en) * | 2010-03-31 | 2015-02-04 | 日本碍子株式会社 | Honeycomb structure |
| JP5170164B2 (en) * | 2010-06-11 | 2013-03-27 | 株式会社デンソー | Electric heating type catalyst equipment |
| US8545610B2 (en) * | 2010-07-30 | 2013-10-01 | Aisan Kogyo Kabushiki Kaisha | Fuel vapor treating apparatuses having a high thermal conductive honeycomb core |
| JP5883299B2 (en) * | 2011-03-24 | 2016-03-09 | 日本碍子株式会社 | Heater for heating lubricating fluid |
| JP6740995B2 (en) * | 2017-06-30 | 2020-08-19 | 株式会社デンソー | Electric resistor, honeycomb structure, and electrically heated catalyst device |
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2021
- 2021-11-19 US US17/455,700 patent/US20220287154A1/en active Pending
- 2021-12-01 DE DE102021213628.1A patent/DE102021213628A1/en active Pending
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| DE102021213628A1 (en) | 2022-09-08 |
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